The objective of carbon dioxide capture is to address the increasing problem of the effects of the emission of carbon dioxide (a greenhouse gas) into the atmosphere, by separating carbon dioxide from gaseous products of various processes, and deliver the separated carbon dioxide for further use, processing, and storage. Recently, the possibility of underground storage in deep geological formations has been given much consideration, but the economic and practical difficulties in separating the carbon dioxide from mixed gas streams have not been satisfactorily addressed.
Currently, there are three main approaches to capturing carbon dioxide from the combustion of fossil fuels, namely, pre-combustion capture, postcombustion capture, and oxy-fuel combustion. For a conventional air-fired coal power plant, where the normal carbon dioxide concentration in the boiler exit flue gas could be around 15% by volume, post-combustion capture may be an appropriate option. In this process, the carbon dioxide from the flue gas can be removed by scrubbing with chemical solvents, such as an amine solution, or various sorbents. However, advanced technologies such as gasification or oxy-fuel combustion can make possible alternative means of carbon dioxide capture. For a gasification system, the carbon dioxide can be more effectively removed using pre-combustion capture systems using physical solvents or membrane technology. Oxy-fuel combustion provides an advantageous approach to carbon dioxide capture, whereby combustion takes place in an oxygen-enriched environment, thus producing a flue gas stream which is rich in carbon dioxide, and thus can readily be captured and compressed using non-solvent based processes, such as low-temperature gas separation, for pipeline transport. The selection of an appropriate carbon dioxide capture process for a particular application thus depends on several factors including the combustion technology adopted, the flue gas composition and condition, and the end-user's requirement.
Known processes for carbon dioxide capture and subsequent purification via a compression and cooling system have been primarily confined to applications in the food industry and some chemical plant applications. In many of these applications, the concentration of carbon dioxide in the inlet gas stream is often greater than 90% and relatively free from the sort of contaminates typical of most combustion processes, e.g. SOx and NOx. A typical capture plant consists of a pre-cleaning stage, a compression stage and a liquefaction stage. In the pre-cleaning stage the inlet gas stream is cleaned of solid particles and/or impurities such as mercury, SOx, etc., and then is passed through an initial demister unit before entering the compression stage. In the compression stage, the gas stream is compressed, cooled (which may be in multiple stages and forms condensates that can be removed in condensate separator vessels), and then passed through a drier, to further dry the gas stream. In the liquefaction stage, the gas stream is further cooled for liquefying the carbon dioxide and separating it from non-condensable gases to form the carbon dioxide product stream. The non-condensable gases such as argon and oxygen or nitrogen, are vented along with a small percentage of carbon dioxide in gaseous form to the atmosphere. Some systems partially vent non-condensable gases through the dryer to assist regeneration of the dryer material. Depending on the downstream process, the carbon dioxide may be sent to insulated storage tanks, used directly, or transported in a pipeline or other means of transportation for underground storage.
For the separation of carbon dioxide from the flue gas streams of fossil energy conversion systes, various different processes are known and used. These processes currently include the use of membranes, chemical and physical solvents, sorbents, cryogenic or low-temperature separation. The main factors involved in the selection of a suitable separation process include the energy conversion system, the concentration of carbon dioxide expected in the flue gas stream, the purity requirement of the carbon dioxide product stream, the energy consumption, and the cost and efficiency of capture. For flue gas streams with higher concentrations of carbon dioxide, the preferred approach is to use a process including the low temperature separation of gas mixtures. This can be done through a simple multi-stage direct compression and cooling process, or more complex processes that might involve different ways of cooling, compression or recycling of the flue gas to liquefy and separate the carbon dioxide from other gases.
However, each of these processes suffers from various disadvantages, in particular the complexity of the systems and the size of the equipment, or the amount of energy required, and thus the capital and operation costs of the additional plant components, and the costs associated with providing the necessary energy for refrigeration.
It has now been found that a system can be provided for more efficient and cost-effective separation of carbon dioxide from carbon dioxide rich gas streams emitted from fossil fuel and other industrial plants using a new low-temperature gas separation process that includes both auto-refrigeration and gas recycling. In particular, it has been found that an approach can be selected which provides compression to the inlet gas streams in multiple stages with inter-stage cooling and condensate removal, while using the energy in the compressed gas to provide cooling to the incoming stream, and at the same time using an expansion stage before recycling a portion of the gas back to the compressor, at some intermediate stage within the multiple compression stages. It has further been found that a novel arrangement of process flow pathways can be provided with respect to separation vessels, multi-pass heat exchangers, gas recycle pathways, and gas throttling to reduce the overall energy demand and temperature of the process without the use of external refrigeration means, in a simple and compact system, without the disadvantages of known processes and systems.